Atmospheric carbon dioxide levels recently surpassed 400 ppm, the highest concentration seen on the Earth in over three million years. These record levels and the rate at which these levels are increasing are due in large part to anthropogenic emissions from the combustion of fossil fuels. Therefore, reducing CO2 emissions and using carbon-neutral fuels is of paramount importance for society. The transportation sector is an especially important target, as 27% of overall greenhouse gas emissions are from automobiles. Replacing fossil fuels with a carbon-neutral fuel such as hydrogen or natural gas (methane) would be advantageous due to hydrogen's high gravimetric energy content, clean combustion, and potential renewability and the higher amount of energy derived from natural gas per unit of CO2 emitted. The widespread adoption of hydrogen and methane as fuels, however, is limited because they are gases at room temperature and pressure. Most efforts to increase the volumetric energy density of these gases in fuel tanks have relied on cryogenic storage and/or compression, but these strategies have proven too costly for the widespread adoption of either for fueling motor vehicles. Large cooling and compressing systems contribute additional unwanted mass to motor vehicles and require a significant energetic cost to store hydrogen at a useful density. Alternatively, solid adsorbents provide promise as a way to store H2 at high densities while simultaneously using lower pressures and higher temperatures than are currently employed. The U.S. Department of Energy (DOE) has set targets for on-board H2 storage of 5.5 wt % gravimetric capacity, 40 g/L volumetric capacity, a temperature range of −40 to 60° C., and a maximum delivery pressure of 100 atm. Unfortunately, currently available adsorbents do not have the requisite capacities at relevant temperatures and pressures. Furthermore, binding enthalpies in the range of −15 to −20 kJ/mol are necessary for practical H2 storage and have yet to be achieved, leading to the need for further development of solid porous adsorbents for H2 storage.